A two-step ligand-exchange strategy is developed, in which the long-carbon- chain ligands on all-inorganic perovskite (CsPbX , X = Br, Cl) quantum dots (QDs) are replaced with halide-ion-pair ligands. Green and blue light-emitting diodes made from the halide-ion-pair-capped quantum dots exhibit high external quantum efficiencies compared with the untreated QDs.
Although halide perovskite nanocrystals (NCs) are promising materials for optoelectronic devices, they suffer severely from chemical and phase instabilities. Moreover, the common capping ligands like oleic acid and oleylamine that encapsulate the NCs will form an insulating layer, precluding their utility in optoelectronic devices. To overcome these limitations, we develop a postsynthesis passivation process for CsPbI NCs by using a bidentate ligand, namely 2,2'-iminodibenzoic acid. Our passivated NCs exhibit narrow red photoluminescence with exceptional quantum yield (close to unity) and substantially improved stability. The passivated NCs enabled us to realize red light-emitting diodes (LEDs) with 5.02% external quantum efficiency and 748 cd/m luminance, surpassing by far LEDs made from the nonpassivated NCs.
Colloidal quantum dots (CQDs) offer promise in flexible electronics, light sensing and energy conversion. These applications rely on rectifying junctions that require the creation of high-quality CQD solids that are controllably n-type (electron-rich) or p-type (hole-rich). Unfortunately, n-type semiconductors made using soft matter are notoriously prone to oxidation within minutes of air exposure. Here we report high-performance, air-stable n-type CQD solids. Using density functional theory we identify inorganic passivants that bind strongly to the CQD surface and repel oxidative attack. A materials processing strategy that wards off strong protic attack by polar solvents enabled the synthesis of an air-stable n-type PbS CQD solid. This material was used to build an air-processed inverted quantum junction device, which shows the highest current density from any CQD solar cell and a solar power conversion efficiency as high as 8%. We also feature the n-type CQD solid in the rapid, sensitive, and specific detection of atmospheric NO2. This work paves the way for new families of electronic devices that leverage air-stable quantum-tuned materials.
So-called zero-dimensional perovskites, such as Cs 4 PbBr 6 , promise outstanding emissive properties. However, Cs 4 PbBr 6 is mostly prepared by melting of precursors that usually leads to a coformation of undesired phases. Here, we report a simple low-temperature solution-processed synthesis of pure Cs 4 PbBr 6 with remarkable emission properties. We found that pure Cs 4 PbBr 6 in solid form exhibits a 45% photoluminescence quantum yield (PLQY), in contrast to its three-dimensional counterpart, CsPbBr 3 , which exhibits more than 2 orders of magnitude lower PLQY. Such a PLQY of Cs 4 PbBr 6 is significantly higher than that of other solid forms of lower-dimensional metal halide perovskite derivatives and perovskite nanocrystals. We attribute this dramatic increase in PL to the high exciton binding energy, which we estimate to be ∼353 meV, likely induced by the unique Bergerhoff−Schmitz−Dumont-type crystal structure of Cs 4 PbBr 6 , in which metal-halide-comprised octahedra are spatially confined. Our findings bring this class of perovskite derivatives to the forefront of color-converting and light-emitting applications.
Organo-metal halide perovskites are a promising platform for optoelectronic applications in view of their excellent charge transport and bandgap tunability. However, their low photoluminescence quantum efficiencies, especially in low excitation regimes, limit their efficiency for light emission. Consequently, perovskite light emitting devices are operated under high injection, a regime under which the materials have so far been unstable. Here we show that, by concentrating photoexcited states into a small subpopulation of radiative domains, one can achieve a high quantum yield even at low excitation intensities. We tailor the composition of quasi-2D perovskites to direct energy transfer into the lowest-bandgap
We demonstrate ultra-air- and photostable CsPbBr3 quantum dots (QDs) by using an inorganic-organic hybrid ion pair as the capping ligand. This passivation approach to perovskite QDs yields high photoluminescence quantum yield with unprecedented operational stability in ambient conditions (60 ± 5% lab humidity) and high pump fluences, thus overcoming one of the greatest challenges impeding the development of perovskite-based applications. Due to the robustness of passivated perovskite QDs, we were able to induce ultrastable amplified spontaneous emission (ASE) in solution processed QD films not only through one photon but also through two-photon absorption processes. The latter has not been observed before in the family of perovskite materials. More importantly, passivated perovskite QD films showed remarkable photostability under continuous pulsed laser excitation in ambient conditions for at least 34 h (corresponds to 1.2 × 10(8) laser shots), substantially exceeding the stability of other colloidal QD systems in which ASE has been observed.
Cesium lead halide perovskite quantum dots (PQDs) have attracted significant interest for optoelectronic applications in view of their high brightness and narrow emission linewidth at visible wavelengths. A remaining challenge is the degradation of PQDs during purification from the synthesis solution.This is attributed to proton transfer between oleic acid and oleylamine surface capping agents that leads to facile ligand loss. Here, a new synthetic method is reported that enhances the colloidal stability of PQDs by capping them solely using oleic acid (OA). Quaternary alkylammonium halides are used as precursors, eliminating the need for oleylamine. This strategy enhances the colloidal stability of OA capped PQDs during purification, allowing us to remove excess organic content in thin films. Inverted red, green, and blue PQD light-emitting diodes (LED) are fabricated for the first time with solution-processed polymerbased hole transport layers due to higher robustness of OA capped PQDs to solution processing. The blue and green LEDs exhibit threefold and tenfold improved external quantum efficiency (EQE), respectively, compared to prior related reports for amine/ammonium capped cross-linked PQDs. The brightest blue LED based on all inorganic CsPb(Br 1−x Cl x ) 3 PQDs is also reported. Figure 5. a) Transient absorption spectra for green-emitting PQDs in toluene solution for several pump intensities (inset shows the multiexciton dynamics at high excitation energy (〈N〉 = 2.2)). b) Comparison between the transient absorption spectra of PQDs in solution and film. full paper 8763 wileyonlinelibrary.com
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